科研成果 by Year: 2021

2021
Cheng X, Chen Q, Li Y, Huang G, Liu Y, Lu S, Zheng Y, Qiu W, Lu K, Qiu X, et al. Secondary Production of Gaseous Nitrated Phenols in Polluted Urban Environments. Environmental Science & Technology. 2021.
Gkatzelis GI, Papanastasiou DK, Karydis VA, Hohaus T, Liu Y, Schmitt SH, Schlag P, Fuchs H, Novelli A, Chen Q, et al. Uptake of water-soluble gas-phase oxidation products drives organic particulate pollution in Beijing. Geophysical Research Letters. 2021;n/a:e2020GL091351.Abstract
Abstract Despite the recent decrease in pollution events in Chinese urban areas, the World Health Organization air quality guideline values are still exceeded. Observations from monitoring networks show a stronger decrease of organic aerosol directly emitted to the atmosphere relative to secondary organic aerosol (SOA) generated from oxidation processes. Here, the uptake of water-soluble gas-phase oxidation products is reported as a major SOA contribution to particulate pollution in Beijing, triggered by the increase of aerosol liquid water. In pollution episodes, this pathway is enough to explain the increase in SOA mass, with formaldehyde, acetaldehyde, glycolaldehyde, formic, and acetic acid alone explaining 15 to 25% of the SOA increase. Future mitigation strategies to reduce non-methane volatile organic compound emissions should be considered to reduce organic particulate pollution in China.
Yan C, Yin R, Lu Y, Dada L, Yang D, Fu Y, Kontkanen J, Deng C, Garmash O, Ruan J, et al. The synergistic role of sulfuric acid, bases, and oxidized organics governing new-particle formation in Beijing. Geophysical Research Letters. 2021;n/a:e2020GL091944.Abstract
Abstract Intense and frequent new particle formation (NPF) events have been observed in polluted urban environments, yet the dominant mechanisms are still under debate. To understand the key species and governing processes of NPF in polluted urban environments, we conducted comprehensive measurements in downtown Beijing during January – March 2018. We performed detailed analyses on sulfuric acid cluster composition and budget, as well as the chemical and physical properties of oxidized organic molecules. Our results demonstrate that the fast clustering of sulfuric acid (H2SO4) and base molecules triggered the NPF events, and oxidized organic molecules (OOMs) further helped grow the newly formed particles towards climate- and health-relevant sizes. This synergistic role of H2SO4, base species, and OOMs in NPF is likely representative of polluted urban environments where abundant H2SO4 and base species usually co-exist, and OOMs are with moderately low volatility when produced under high NOx concentrations.
Song M, Li X, Yang S, Yu X, Zhou S, Yang Y, Chen S, Dong H, Liao K, Chen Q, et al. Spatiotemporal variation, sources, and secondary transformation potential of volatile organic compounds in Xi'an, China. Atmospheric Chemistry and Physics. 2021;21:4939-4958.
Yuan W, Huang RJ, Yang L, Wang T, Duan J, Guo J, Ni H, Chen Y, Chen Q, Li Y, et al. Measurement report: PM2.5-bound nitrated aromatic compounds in Xi'an, Northwest China – seasonal variations and contributions to optical properties of brown carbon. Atmospheric Chemistry and Physics. 2021;21:3685-3697.
Liu Z, Zhou M, Chen Y, Chen D, Pan Y, Song T, Ji D, Chen Q, Zhang L. The nonlinear response of fine particulate matter pollution to ammonia emission reductions in North China. Environmental Research Letters. 2021.Abstract
Recent Chinese air pollution actions have significantly lowered the levels of fine particulate matter (PM2.5) in North China via controlling emissions of sulfur dioxide (SO2) and nitrogen oxides (NO x ) together with primary aerosols, while the emissions of another precursor, ammonia (NH3), have not yet been regulated. This raises a question that how effective the NH3 emission controls can be on the mitigation of PM2.5 pollution along with the reduction of SO2 and NO x emissions. Here we use a regional air quality model to investigate this issue focusing on the PM2.5 pollution in North China for January and July 2015. We find that the efficiency of the PM2.5 reduction is highly sensitive to the NH3 emission and its reduction intensity. Reductions in the population-weighted PM2.5 concentration (PWC) in the Beijing–Tianjin–Hebei region are only 1.4–3.8 μg m−3 (1.1%–2.9% of PM2.5) with 20%–40% NH3 emission reductions, but could reach 8.1–26.7 μg m−3 (6.2%–21%) with 60%–100% NH3 emission reductions in January 2015. Besides, the 2015–2017 emission changes (mainly reduction in SO2 emissions) could lower the PM2.5 control efficiency driven by the NH3 reduction by up to 30% for high NH3 emission conditions, while lead to no change or increase in the efficiency when NH3 emissions become low. NO x emission reductions may enhance the wintertime PM2.5 pollution due to the weakened titration effect and can be offset by simultaneously controlling NH3 emissions. Our results emphasize the need to jointly consider NH3 with SO2 and NO x emission controls when designing PM2.5 pollution mitigation strategies.
Li Y, Liu B, Ye J, Jia T, Khuzestani RB, Sun JY, Cheng X, Zheng Y, Li X, Wu C, et al. Unmanned Aerial Vehicle Measurements of Volatile Organic Compounds over a Subtropical Forest in China and Implications for Emission Heterogeneity. ACS Earth and Space Chemistry. 2021;5:247-256.
Shi X, Qiu X, Chen Q, Chen S, Hu M, Rudich Y, Zhu T. Organic Iodine Compounds in Fine Particulate Matter from a Continental Urban Region: Insights into Secondary Formation in the Atmosphere. Environmental Science & Technology. 2021;55:1508-1514.
Mehra A, Canagaratna M, Bannan TJ, Worrall SD, Bacak A, Priestley M, Liu D, Zhao J, Xu W, Sun Y, et al. Using highly time-resolved online mass spectrometry to examine biogenic and anthropogenic contributions to organic aerosol in Beijing. Faraday Discussions. 2021.Abstract
Organic aerosols, a major constituent of fine particulate mass in megacities, can be directly emitted or formed from secondary processing of biogenic and anthropogenic volatile organic compound emissions. The complexity of volatile organic compound emission sources, speciation and oxidation pathways leads to uncertainties in the key sources and chemistry leading to formation of organic aerosol in urban areas. Historically, online measurements of organic aerosol composition have been unable to resolve specific markers of volatile organic compound oxidation, while offline analysis of markers focus on a small proportion of organic aerosol and lack the time resolution to carry out detailed statistical analysis required to study the dynamic changes in aerosol sources and chemistry. Here we use data collected as part of the joint UK–China Air Pollution and Human Health (APHH-Beijing) collaboration during a field campaign in urban Beijing in the summer of 2017 alongside laboratory measurements of secondary organic aerosol from oxidation of key aromatic precursors (1,3,5-trimethyl benzene, 1,2,4-trimethyl benzene, propyl benzene, isopropyl benzene and 1-methyl naphthalene) to study the anthropogenic and biogenic contributions to organic aerosol. For the first time in Beijing, this study applies positive matrix factorisation to online measurements of organic aerosol composition from a time-of-flight iodide chemical ionisation mass spectrometer fitted with a filter inlet for gases and aerosols (FIGAERO-ToF-I-CIMS). This approach identifies the real-time variations in sources and oxidation processes influencing aerosol composition at a near-molecular level. We identify eight factors with distinct temporal variability, highlighting episodic differences in OA composition attributed to regional influences and in situ formation. These have average carbon numbers ranging from C5–C9 and can be associated with oxidation of anthropogenic aromatic hydrocarbons alongside biogenic emissions of isoprene, α-pinene and sesquiterpenes.